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The effects of the cell parameter and chemical composition on the surface charge properties of five kinds of different colour montmorillonites were studied. The results indicate that the surface isoelectric point(IEP) of the montmorillonite shows positive correlation with the mass fractions of Fe2O3 and K20, but it has little relation to the mass fractions of other chemical compositions. At around pH=6.8, the surface zeta potential of the montmorillonite shows the negative relationship with the mass fractions of Fe2O3 and MgO, but it does not linearly correlate to the mass fractions of other chemical compositions. Cell parameter(b0) of the montmofillonite expresses negative linear relationship with mass fractions of K2O and Na2O, so does c0sinβ with mass fractions of SiO2 and Fe2O3. And there is no specific relationship between bo and IEP of different montmori Uonites, but there is positive correlation between c0sinβ and IEP of different montmorillonite samples.